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Search indexed NASA NTRS and DOE OSTI research on propulsion, heat transfer, battery materials and energy systems. Follow report and document links to the original sources.

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At least 955 records · Page 53
All sourcesNASA NTRSDOE OSTI
DOE OSTI2022

A comparison of neural network architectures for data-driven reduced-order modeling

The popularity of deep convolutional autoencoders (CAEs) has engendered new and effective reduced-order models (ROMs) for the simulation of large-scale dynamical systems. Despite this, it is still unknown whether deep CAEs provide superior performance over established linear techniques or other network-based methods in all modeling scenarios. To elucidate this, the effect of autoencoder architecture on its associated ROM is studied through the comparison of deep CAEs against two alternatives: a simple fully connected autoencoder, and a novel graph convolutional autoencoder. Through benchmark experiments, it is shown that the superior autoencoder architecture for a given ROM application is highly dependent on the size of the latent space and the structure of the snapshot data, with the proposed architecture demonstrating benefits on data with irregular connectivity when the latent space is sufficiently large.

42 ENGINEERING↗
DOE OSTI2022

Residual Stress Modeling and Advanced Diffraction Measurements of 347H Steel Weldments

The 347H stainless steel is a primary high-temperature material for many energy and power generation industries. Stress relief cracking (SRC) has been a particular concern in welding of this material. The residual stress induced by welding and its evolution during post-welding heat treatment (PWHT) and subsequent operating and service conditions is one of the primary factors contributing to SRC. The lifetime of welded structure components is also controlled by the precipitation kinetics that accompanies PWHT, stress relaxation process, and long-term aging and complex synergistic factors. Various theories have been proposed in the past to explain SRC. However, a widely accepted approach to predicting the entire damage evolution and the resulting performance reduction is still lacking. This study is to demonstrate a reliable solution for two critical issues that affect the predictions. First, the residual stress distribution obtained from both simulation and neutron diffraction is compared, which increases the accuracy of mechanical analysis simulation model and therefore builds a solid basis for the lifetime prediction model. Second, the generation, evolution, and annihilation of precipitates are monitored by the synchrotron diffraction experiment. Preliminary results demonstrate the critical importance of precipitation kinetics on the residual stress distribution/redistribution during heat treatments.

Yang, Yi↗
DOE OSTI2014

Plasma response measurements of non-axisymmetric magnetic perturbations on DIII-D via soft x-ray imaging

Recent observations on DIII-D have advanced the understanding of plasma response to applied resonant magnetic perturbations (RMPs) in both H-mode and L-mode plasmas. Three distinct 3D features localized in minor radius are imaged via filtered soft x-ray emission: (i) the formation of lobes extending from the unperturbed separatrix in the X-point region at the plasma boundary, (ii) helical kink-like perturbations in the steep-gradient region inside the separatrix, and (iii) amplified islands in the core of a low-rotation L-mode plasma. In this study, these measurements are used to test and to validate plasma response models, which are crucial for providing predictive capability of edge-localized mode control. In particular, vacuum and two-fluid resistive magnetohydrodynamic(MHD) responses are tested in the regions of these measurements. At the plasma boundary in H-mode discharges with n = 3 RMPs applied, measurements compare well to vacuum-field calculations that predict lobe structures. Yet in the steep-gradient region, measurements agree better with calculations from the linear resistive two-fluid MHD code, M3D-C1. Relative to the vacuum fields, the resistive two-fluid MHD calculations show a reduction in the pitch-resonant components of the normal magnetic field (screening), and amplification of non-resonant components associated with ideal kink modes. However, the calculations still over-predict the amplitude of the measuredperturbation by a factor of 4. In a slowly rotating L-mode plasma with n = 1 RMPs, core islands are observed amplified from vacuum predictions. Finally, these results indicate that while the vacuum approach describes measurements in the edge region well, it is important to include effects of extended MHD in the pedestal and deeper in the plasma core.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗
DOE OSTI2023

Investigating the Electronic Structure of Prospective Water-Splitting Oxide BaCe 0.25 Mn 0.75 O 3-δ before and after Thermal Reduction

BaCe 0.25 Mn 0.75 O 3-δ (BCM), a non-stoichiometric oxide with a layered perovskite-like crystal structure, has recently emerged as a prospective contender for application in renewable energy harvesting by solar thermochemical hydrogen generation. Using solar-thermal energy and a reducing environment, oxygen vacancies can be created in high-temperature BCM, and the reduced crystal so obtained can, in turn, produce H 2 by stripping oxygen from H 2 O. Therefore, a first step toward understanding the working mechanism and optimizing the performance of BCM is a thorough and comparative analysis of the electronic structure of the pristine and the reduced material. In this paper, we probe the electronic structure of BCM using the combined effort of first-principles calculations and experimental O K-edge X-ray absorption spectroscopy (XAS). The computed projected density of states (PDOS) and orbital plots are used to propose a simplified model for orbital mixing between the oxygen and metal atoms. With the help of state-of-the-art simulations, we are able to find the origins of the XAS peaks and categorize them on the basis of contribution from Ce and Mn. For the reduced crystal, the calculations show that the change in electron density resulting from the reduction is strongly localized around the oxygen vacancy. Experimental measurements reveal a marked lowering of the first O K-edge peak in the reduced crystal. Using theoretical analysis, this is shown to result from lifting of spin degeneracy in the absorption peaks as well as from a diminished O 2p contribution to the frontier unoccupied orbitals, in accordance with the tight binding scheme. The simulated results serve as a reference for the extent of spectral change as a function of the percentage of oxygen vacancies in the reduced crystal. Here, our study paves the way for the investigation of the working mechanism of BCM and for computational and experimental efforts aimed at design and discovery of efficient water-splitting oxides.

08 HYDROGEN↗
DOE OSTI2016

Comprehensive characterization of ball-milled powders simulating a tribofilm system

A model system was used to simulate the properties of tribofilms which form during automotive braking. The model system was prepared by ball milling of a blend of 70 vol.% iron oxides, 15 vol.% molybdenum disulfide and 15 vol.% graphite. The resulting mixture was characterized by X-ray powder diffraction (XRD), X-ray photoelectron spectroscopy (XPS), and various transmission electron microscopic (TEM) methods, including energy dispersive X-ray spectroscopy (EDXS), high resolution investigations (HRTEM) with corresponding simulation of the HRTEM images, diffraction methods such as scanning nano-beam electron diffraction (SNBED) and selected area electron diffraction (SAED). It could be shown that the ball milling caused a reduction of the grain size of the initial components to the nanometer range. Sometimes even amorphization or partial break-down of the crystal structure was observed for MoS{sub 2} and graphite. Moreover, chemical reactions lead to a formation of surface coverings of the nanoparticles by amorphous material, molybdenum oxides, and iron sulfates as derived from XPS. - Highlights: • Ball milling of iron oxides, MoS{sub 2}, and graphite to simulate a tribofilm • Increasing coefficient of friction after ball milling of the model blend • Drastically change of the diffraction pattern of the powder mixture • TEM & XPS showed the components of the milled mixture and the process during milling. • MoS{sub 2} and graphite suffered a loss in translation symmetry or became amorphous.

36 MATERIALS SCIENCE↗
DOE OSTI2025

Engineering spin coherence in core-shell diamond nanocrystals

Fluorescent diamond nanocrystals can host spin qubit sensors capable of probing the physical properties of biological systems with nanoscale spatial resolution. Sub-100 nm diamond nanosensors can readily be delivered into intact cells and even living organisms. However, applications beyond current proof-of-principle experiments require a substantial increase in sensitivity, which is limited by surface induced charge instability and electron-spin dephasing. In this work, we utilize engineered core-shell structures to achieve a drastic increase in qubit coherence times (T 2 ) from 1.1 to 35 μs in bare nanodiamonds to upward of 52 to 87 μs. We use electron-paramagnetic-resonance results to present a band bending model and connect silica encapsulation to the removal of deleterious mid-gap surface states that are negatively affecting the qubit’s spin properties. Combined with a 1.9-fold increase in particle luminescence these advances correspond to up to two-order-of-magnitude reduction in integration time. Probing qubit dynamics at a single particle level further reveals that the noise characteristics fundamentally change from a bath with spins that rearrange their spatial configuration during the course of an experiment to a more dilute static bath. The observed results shed light on the underlying mechanisms governing fluorescence and spin properties in diamond nanocrystals and offer an effective noise mitigation strategy based on engineered core-shell structures.

core-shell↗
DOE OSTI2023

Influence of clay mineral weathering on green rust formation at iron-reducing conditions

Green rusts (GR) are important drivers for trace metal and nutrient cycling in suboxic environments. We investigated whether green rusts would incorporate aluminum (Al) or other elements from naturally-formed clay minerals containing easily-weatherable clay minerals (e.g. mica, interlayered clays). We isolated the clay minerals from a Matapeake silt loam soil by removal of silt and sand, organic matter, and reducible oxides to study mechanisms of interaction between Fe(II) and soil-sourced clay minerals. We conducted batch Fe(II) sorption experiments at multiple near-neutral pHs (6.5–7.5) and reaction times (2h–365 days). Mineral transformations were characterized by selective extractions, X-ray diffraction (XRD), and Fe X-ray absorption spectroscopy (XAS) analyzed by shell-fitting and linear combination fitting (LCF) with natural and synthetic standards. Clay mineral fraction contained a mixture of quartz, kaolinite, interlayered vermiculite, mica, and chlorite with significant structural Fe (2.6% wt). Uptake of Fe(II) increased with pH and kinetics were rapid until 5 days, followed by slow continuous Fe(II) uptake. Citrate-bicarbonate desorption kinetics from Fe(II) sorbed clay released more Al and silicon (Si) compared with unreacted soil clay fraction whereas magnesium (Mg) and potassium (K) were unaffected. Citrate-bicarbonate extracted Fe contained more Fe(II) than an ideal GR with an Fe(II)/Fe(III) molar ratio of 5.50. Analysis of the Fe EXAFS by both LCF and shell fitting was best modeled as a combination of Fe(III)-clay reduction to Fe(II) and precipitation of GR and Fe(II)-Al LDH. After 7 days of Fe(II) sorption, LCF identified 55.2% total Fe in clay, 33.4% GR(Cl) and 11.4% Fe(II)-Al LDH. Further, these results provide novel evidence of Fe(II)-Al LDHs precipitating on naturally-formed soil clay minerals as a minor phase to GR. The geochemical implications are that GRs formed in soils and sediments should be considered to have Al and Si as well as Mg substitutions affecting their structure and reactivity.

58 GEOSCIENCES↗
DOE OSTI2016

Linking structure to function: The search for active sites in non-platinum group metal oxygen reduction reaction catalysts

Atomic-scale structures of oxygen reduction reaction (ORR) active sites in non-platinum group metal (non-PGM) catalysts, made from pyrolysis of carbon, nitrogen, and transition-metal (TM) precursors have been the subject of continuing discussion in the fuel cell electrocatalysis research community. We found that quantum chemical modeling is a path forward for understanding of these materials and how they catalyze the ORR. Here, we demonstrate through literature examples of how such modeling can be used to better understand non-PGM ORR active site relative stability and activity and how such efforts can also aid in the interpretation of experimental signatures produced by these materials.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2018

Experimental and theoretical insight into the soot tendencies of the methylcyclohexene isomers

The formation of soot precursors during combustion of three positional isomers of methylcyclohexene was investigated in flow reactor experiments and through density functional theory simulations. As evidenced by a recently published structure-property model, the sooting tendencies of these compounds differ from those of structurally similar molecules - suggesting new or unusual reaction chemistry. It was demonstrated that 1-methyl-1-cyclohexene and 4-methyl-1-cyclohexene preferentially react via a retro-Diels-Alder pathway leading to ring opening and molecular weight reduction. 3-methyl-1-cyclohexene, which exhibits much higher yield sooting index, preferentially reacts via dehydrogenation to cyclohexadienes and toluene - consistent with higher soot formation. It was demonstrated that the relative stability of the first radical intermediate plays a considerable role in determining the branching ratio between formation of soot precursors and ring opened retro-Diels-Alder reaction products. This study underscores the importance that small structural features can have in determining the ultimate fate of carbon during combustion processes.

09 BIOMASS FUELS↗
DOE OSTI2017

Characterization of Silicon Nanocrystal Surfaces by Multidimensional Solid-State NMR Spectroscopy

The chemical and photophysical properties of silicon nanocrystals (Si NCs) are strongly dependent on the chemical composition and structure of their surfaces. Here we use fast magic angle spinning (MAS) and proton detection to enable the rapid acquisition of dipolar and scalar 2D 1 H– 29 Si heteronuclear correlation (HETCOR) solid-state NMR spectra and reveal a molecular picture of hydride-terminated and alkyl-functionalized surfaces of Si NCs produced in a nonthermal plasma. 2D 1 H– 29 Si HETCOR and dipolar 2D 1 H– 1 H multiple-quantum correlation spectra illustrate that resonances from surface mono-, di-, and trihydride groups cannot be resolved, contrary to previous literature assignments. Instead the 2D NMR spectra illustrate that there is large distribution of 1 H and 29 Si chemical shifts for the surface hydride species in both the as-synthesized and functionalized Si NCs. However, proton-detected 1 H– 29 Si refocused INEPT experiments can be used to unambiguously differentiate NMR signals from the different surface hydrides. Varying the 29 Si evolution time in refocused INEPT experiments and fitting the oscillation of the NMR signals allows for the relative populations of the different surface hydrides to be estimated. This analysis confirms that monohydride species are the predominant surface species on the as-synthesized Si NCs. A reduction in the populations of the di- and trihydrides is observed upon functionalization with alkyl groups, consistent with our previous hypothesis that the trihydride, or silyl (*SiH 3 ), group is primarily responsible for initiating surface functionalization reactions. Density functional theory (DFT) calculations were used to obtain quantum chemical structural models of the Si NC surface and reproduce the observed 1 H and 29 Si chemical shifts. Furthermore, the approaches outlined here will be useful to obtain a more detailed picture of surface structures for Si NCs and other hydride-passivated nanomaterials.

29Si NMR↗
DOE OSTI2019

Lattice Expansion in Hybrid Perovskites: Effect on Optoelectronic Properties and Charge Carrier Dynamics

Hybrid halide perovskites frequently undergo structural expansion which significantly affects their electronic properties and in particular charge carrier dynamics. Various stimuli such as residual strain, light illumination, compositional engineering may deform the soft lattices of these materials. It is essential to atomistically model how geometric changes modify electronic characteristics important for applications such as light harvesting or lighting. Using ab initio simulations, here we investigate the structural dynamics and optoelectronic properties of FAPbI 3 under tensile strain. The applied strain leads to elongation of the Pb-I bonds and a reduction of PbI 6 octahedra tilting, which manifests as a blue-shifts in band gaps. Nonadiabatic molecular dynamics simulations further reveal that charge carrier recombination rates moderately slow down in these expanded lattices. Complex influences of lattice dynamics on elastic and inelastic electron-phonon scattering results in longer carrier lifetime which is advantageous for efficient solar cells. By providing detailed information on the structure-property relationships, this work emphasizes the role of controlled lattice expansion on enhancing the electronic functionalities of hybrid perovskites.

36 MATERIALS SCIENCE↗
DOE OSTI2015

Simulation of Defect Reduction in Block Copolymer Thin Films by Solvent Annealing

Solvent annealing provides an effective means to control the self-assembly of block copolymer (BCP) thin films. Multiple effects, including swelling, shrinkage, and morphological transitions, act in concert to yield ordered or disordered structures. The current understanding of these processes is limited; by relying on a theoretically informed coarse-grained model of block copolymers, a conceptual framework is presented that permits prediction and rationalization of experimentally observed behaviors. Through proper selection of several process conditions, it is shown that a narrow window of solvent pressures exists over which one can direct a BCP material to form well-ordered, defect-free structures.

Hur, Su-Mi↗
DOE OSTI2025

Divertor shaping with neutral baffling as a solution to the tokamak power exhaust challenge

Exhausting power from the hot fusion core to the plasma-facing components is one fusion energy’s biggest challenges. The MAST Upgrade tokamak uniquely integrates strong containment of neutrals within the exhaust area (divertor) with extreme divertor shaping capability. By systematically altering the divertor shape, this study shows the strongest evidence to date to our knowledge that long-legged divertors with a high magnetic field gradient (total flux expansion) deliver key power exhaust benefits without adversely impacting the hot fusion core. These benefits are already achieved with relatively modest geometry adjustments that are more feasible to integrate in reactor designs. Benefits include reduced target heat loads and improved access to, and stability of, a neutral gas buffer that ‘shields’ the target and enhances power exhaust (detachment). Analysis and model comparisons shows these benefits are obtained by combining multiple shaping aspects: long-legged divertors have expanded plasma-neutral interaction volume that drive reductions in particle and power loads, while total flux expansion enhances detachment access and stability. Containing the neutrals in the exhaust area with physical structures further augments these shaping benefits. These results demonstrate strategic variation in the divertor geometry and magnetic topology is a potential solution to one of fusion’s power exhaust challenge.

magnetically confined plasmas↗
DOE OSTI2017

Redox properties of birnessite from a defect perspective

Significance We propose, and preliminarily confirm with experiments, a theoretical model to understand various structure–performance dependences of layered-structure birnessite as an oxygen evolution reaction (OER) catalyst. Besides the well-accepted importance of Mn(III), we emphasize the critical importance of a nonuniform distribution of Mn(III) to OER catalytic activity. Such a distribution contributes to the reduction of the overpotential by building an internal potential step. We further propose the small polaron as a common concept to link the fields of oxygen evolution catalysis and Li-ion batteries, suggesting a promising candidate space for oxygen evolution reaction catalysts.

36 MATERIALS SCIENCE↗
DOE OSTI2015

The impact of dust evolution and photoevaporation on disk dispersal

Protoplanetary disks are dispersed by viscous evolution and photoevaporation in a few million years; in the interim small, sub-micron-sized dust grains must grow and form planets. The time-varying abundance of small grains in an evolving disk directly affects gas heating by far-ultraviolet (FUV) photons, while dust evolution affects photoevaporation by changing the disk opacity and resulting penetration of FUV photons in the disk. Photoevaporative flows, in turn, selectively carry small dust grains, leaving the larger particles—which decouple, from the gas—behind in the disk. We study these effects by investigating the evolution of a disk subject to viscosity, photoevaporation by EUV, FUV, and X-rays, dust evolution, and radial drift using a one-dimensional (1D) multi-fluid approach (gas + different dust grain sizes) to solve for the evolving surface density distributions. The 1D evolution is augmented by 1+1D models constructed at each epoch to obtain the instantaneous disk structure and determine photoevaporation rates. The implementation of a dust coagulation/fragmentation model results in a marginal decrease in disk lifetimes when compared to models with no dust evolution; the disk lifetime is thus found to be relatively insensitive to the evolving dust opacity. We find that photoevaporation can cause significant reductions in the gas/dust mass ratio in the planet-forming regions of the disk as it evolves, and may result in a corresponding increase in heavy element abundances relative to hydrogen. We discuss implications for theories of planetesimal formation and giant planet formation, including the formation of gas-poor giants. After gas disk dispersal, ∼3×10{sup −4} M {sub ⊙} of mass in solids typically remain, comparable to the solids inventory of our solar system.

79 ASTRONOMY AND ASTROPHYSICS↗
DOE OSTI2018

A Combined Experimental and Theoretical Study of Lithiation Mechanism in ZnFe2O4 Anode Materials

ABSTRACT ZnFe 2 O 4 (ZFO) represents a promising anode material for lithium ion batteries, but there is still a lack of deep understanding of the fundamental reduction mechanism associated with this material. In this paper, the complete visualization of reduction/oxidation products irrespective of their crystallinity was achieved experimentally through a compilation of in situ X-ray diffraction, synchrotron based powder diffraction, and ex-situ X-ray absorption fine structure data. Complementary theoretical modelling study further shed light upon the fundamental understanding of the lithiation mechanism, especially at the early stage from ZnFe 2 O 4 up to Li x ZnFe 2 O 4 (x = 2).

36 MATERIALS SCIENCE↗
DOE OSTI2021

Adaptive Site Management Strategies for the Hanford Central Plateau Groundwater

Adaptive site management (ASM) is a systematic and iterative management approach that can be used to expedite the remediation of large and/or complex sites. ASM is defined as a formal and systematic project or site management approach centered on rigorous site planning and a firm understanding of site conditions and uncertainties, using science and technology to routinely re-evaluate and prioritize site remedial actions and characterization activities. The goal of the approach is to create a framework of structured and continuous planning, implementation, and assessment processes that accommodates new information and changing site conditions to develop effective and efficient cleanup approaches that achieves the required outcome(s) while optimizing costs, cleanup timeframe, and performance. Central to ASM is an evolving conceptual site model (CSM). Over time, incremental reductions in uncertainty associated with the CSM will occur, while supporting continued progress toward site cleanup and closure through remedy optimization and evaluation. ASM has the potential to expedite cleanup for the Central Plateau area at Hanford through a planned and systematic approach for reducing uncertainty with targeted characterization activities, while continuing remediation activities that advance cleanup for key risk-driving contaminants. A core component of cleanup within the Central Plateau is the 200 West Pump-and-Treat (P&T) system. Even with an active P&T remedy, uncertainty exists with respect to plume distributions, total mass in the aquifer, and currently known continuing sources. Additional uncertainty is associated with multiple contaminant source locations in the vadose zone, which have the potential to create new groundwater plumes in the absence of any source control measures, although not all contaminant fluxes to groundwater will result in contaminant concentrations above cleanup levels. Collectively, these uncertainties need to be addressed in the CSM to support effective and efficient site progress toward cleanup goal(s). Other nontechnical factors that may warrant an ASM approach at the Hanford Central Plateau are associated with the formation of operable units (OUs) used to manage cleanup. With the exception of the 200-ZP-1 OU, the three remaining groundwater OUs only have interim action records of decision. Nine vadose zone source area OUs are also in the early stages of the remedial investigation and feasibility study process, with pending characterization and technology identification activities. A set of proposed site objectives for the Central Plateau are provided in this document as an initial consideration/example and basis for discussion for ASM implementation. These example site objectives were selected with the goal of maintaining protectiveness at the Columbia River through confinement of contaminant plumes within an administratively controlled area below existing surface waste sites and waste disposal facilities. Although site decision makers and regulators need to provide concurrence, these site objectives are used in this document to describe the elements of an ASM approach, including selection of interim objectives and a long-term adaptive management plan. Interim objectives are also defined to yield measurable incremental progress toward the overall site goals. This document identifies initial technical considerations for developing an ASM framework for the Central Plateau cleanup decisions. These considerations are intended to facilitate more specific decisions, such as objectives, near- and long-term actions, and performance metrics, to develop an overall approach that maintains protectiveness but recognizes the uncertainty, long timeframe, and technical challenges that need to be considered in selecting, implementing, and managing remediation at the Hanford Central Plateau.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗
DOE OSTI2017

Sediment Transport into the Swinomish Navigation Channel, Puget Sound—Habitat Restoration versus Navigation Maintenance Needs

The 11 mile (1.6 km) Swinomish Federal Navigation Channel provides a safe and short passage to fishing and recreational craft in and out of Northern Puget Sound by connecting Skagit and Padilla Bays, US State abbrev., USA. A network of dikes and jetties were constructed through the Swinomish corridor between 1893 and 1936 to improve navigation functionality. Over the years, these river training dikes and jetties designed to minimize sedimentation in the channel have deteriorated, resulting in reduced protection of the channel. The need to repair or modify dikes/jetties for channel maintenance, however, may conflict with salmon habitat restoration goals aimed at improving access, connectivity and brackish water habitat. Several restoration projects have been proposed in the Skagit delta involving breaching, lowering, or removal of dikes. To assess relative merits of the available alternatives, a hydrodynamic model of the Skagit River estuary was developed using the Finite Volume Community Ocean Model (FVCOM). Here, in this paper, we present the refinement and calibration of the model using oceanographic data collected from the years 2006 and 2009 with a focus on the sediment and brackish water transport from the river and Skagit Bay tide flats to the Swinomish Channel. The model was applied to assess the feasibility of achieving the desired dual outcome of (a) reducing sedimentation and shoaling in the Swinomish Channel and (b) providing a direct migration pathway and improved conveyance of freshwater into the Swinomish Channel. Finally, the potential reduction in shoaling through site-specific structure repairs is evaluated. Similarly, the potential to significantly improve of brackish water habitat through dike breach restoration actions using the McGlinn Causeway project example, along with its impacts on sediment deposition in the Swinomish Navigation Channel, is examined

54 ENVIRONMENTAL SCIENCES↗